A robust <i>in situ</i> adaptive artificial interface for dead-lithium-free lithium metal batteries

The escalating demand for high-performance energy storage, driven by electric vehicles and drones, has intensified research into lithium metal batteries featuring lithium metal anodes. Lithium metal batteries are susceptible to dendrite and dead lithium formation under high current conditions, which impacts their practical applications. This study addresses the challenges of anode stability and dead lithium at high current densities by introducing an inorganic-organic composite artificial solid electrolyte interface (ASEI). We developed a flexible and robust polymer and integrated it with AgNO₃ to <i>in situ</i> generate Ag and Li₃N to form an ASEI. In the ASEI, these inorganic and organic components are <i>in situ</i> generated during the electrochemical process, exhibiting a gradient transition from the solution to the lithium metal interface. This gradient transition of inorganic and organic layers endows the subsequent deposition and dissolution processes with self-adaptive characteristics, allowing for continuous evolution with lithium insertion and extraction. It provides a stable <i>in situ</i> adaptive ASEI that suppresses the formation of dead lithium and dendrites. The lithiophilic properties of Ag, the ionic conductivity of Li₃N and the robustness of the polymers demonstrate superior mechanical strength and electrochemical performance across symmetrical, half, and full cells, showcasing promise for next-generation energy storage solutions.